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Regulating electronic structure of CoN_(4)with axial Co-S for promoting Oxygen reduction and Zn-air battery performance

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Nano Research 2023年第4期16卷 4211-4218页

作者： Chang Chen Zhiqiang Chen Junxi Zhong Xin Song Dongfang Chen Shoujie Liu Weng-Chon Cheong Jiazhan Li Xin Tan Chang He Jiaqi Zhang Di Liu Qiuhua Yuan Chen Chen Qing Peng Yadong Li Department of Chemistry Tsinghua UniversityBeijing 100084China Beijing Key Laboratory of Research and Application for Aerospace Green Propellants Beijing Institute of Aerospace Testing TechnologyBeijing 100048China College of Chemistry and Environmental Engineering Shenzhen UniversityShenzhen 518060China State Key Laboratory of Automtive Safety and Energy Tsinghua UniversityBeijing 100084China Chemistry and Chemical Engineering Guangdong Laboratory Shantou 515031China Department of Physics and Chemistry Faculty of Science and TechnologyUniversity of MacaoMacao 999078China

Regulating the coordination environment of transition-metal based materials in the axial direction with heteroatoms has shown great potential in boosting the Oxygen reduction reaction(ORR).The coordination configuration and the regulation method are pivotal and elusive.Here,we report a combined strategy of matrix-activization and controlled-induction to modify the CoN_(4)site by axial coordination of Co-S(Co1N_(4)-S_(1)),which was validated by the aberration-corrected electron microscopy and X-ray absorption fine structure analysis.The optimal Co1N_(4)-S_(1)exhibits an excellent alkaline ORR activity,according to the half-wave potential(0.897 V vs.reversible hydrogen electrode(RHE)),Tafel slope(24.67 mV/dec),and kinetic current density.Moreover,the Co1N_(4)-S_(1)based Zn-air battery displays a high power density of 187.55 mW/cm^(2)and an outstanding charge-discharge cycling stability for 160 h,demonstrating the promising application potential.Theoretical calculations indicate that the better regulation of CoN_(4)on electronic structure and thus the highly efficient ORR performance can be achieved by axial Co-S.

关键词： electronic structure regulation axial Co-S coordination single-atom Co Oxygen reduction Zn-air battery

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Size and structure tuning of FePt nanoparticles on hollow mesoporous carbon spheres as efficient catalysts for Oxygen reduction reaction

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Rare Metals 2023年第6期42卷 1865-1876页

作者： Cheng Yang Han-Bin Wang Pei Liang Bin-Feng Wu Lei Zhao Ping-Shu Leng Lin Lv Hou-Zhao Wan Hao Wang School of Microelectronics Hubei UniversityWuhan430062China Hubei Yangtze Memory Laboratories Wuhan430205China College of Optical and Electronic Technology China Jiliang UniversityHangzhou310018China

Finding and designing cathode Oxygen reduction reaction(ORR) catalysts with high activity and stability in acidic electrolyte is essential for the large-scale application of fuel cells and metal-air batteries.Pt-based alloys have emerged as potential electrocatalysts for the Oxygen reduction reaction.Herein,we adapted a simple pyrolytic reduction method to grow FePt nanoalloys on hollow mesoporous carbon supports.Benefiting from the ultra-high specific surface of the hollow mesoporous carbon,the in situ formed FePt NPs were homogenously deposited on the carbon supports with size smaller than5 nm.The optimized FePt-HMCS showed a remarkably increased mass activity(MA) of 0.582 A·mg^(-1)_(Pt) at 0.75 V in ORR,being 6.3 times higher than that of commercial Pt/C(0.093 A·mg^(-1)_(Pt)).Meanwhile,the FePt NPs showed negligible decay in mass activity with 21 mV of negative shift in the half-wave potential after 5000 electrochemical cycles,which is more stable than that of commercial Pt/C(6.6% decay in MA with 30 mV of negative shift).The study demonstrated a simple strategy for controlling the alloy size with enhanced metal-support interactions to boost their promising application in fuel cells.

关键词： Oxygen reduction Electrocatalysts Mesoporous carbon FePt alloy

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Molten salt electrochemical modulation of Ni/Co nanoparticles onto N-doped carbon for Oxygen reduction

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Journal of Energy Chemistry 2022年第11期31卷 212-217,I0007页

作者： Xinxin Liang Jialin Chen Biao Hong Tingting Wan Wei Weng Wei Xiao College of Chemistry and Molecular Sciences Hubei Key Laboratory of Electrochemical Power SourcesWuhan UniversityWuhan 430072HubeiChina Zijin School of Geology and Mining Fujian Key Laboratory of Green Extraction and High-value Utilization of Energy MetalsFuzhou UniversityFuzhou 350108FujianChina Queen Marry University of London Engineering School Northwestern Polytechnical UniversityXi’an 710129ShaanxiChina

Activation of oxygen over non-precious materials has been an imperative task to develop efficient electrochemical energy storage and conversion such as fuel cells and metal-air batteries.Herein,a molten salt electrochemical modulation of metal-nitrogen-carbon based compounds(M–N–C)is achieved.By electrochemical treatment of polydopamine-coated NiCo_(2)O_(4)(NiCo_(2)O_(4)@PDA)in molten Li_(2)CO_(3)-Na_(2)CO_(3)-K_(2)CO_(3)at 500℃,Ni/Co bimetal-nitrogen-carbon catalyst(denoted as Ni/Co@NC)consisting of Ni-Co nanoparticles anchoring on porous nitrogen-doped carbon is constructed and evaluated as electrocatalysts towards the Oxygen reduction reaction(ORR).Experimental and calculation results confirm that alloying of Ni-Co and nitrogen doping to carbon enhances the rate-determining transformation of*OH intermediate during ORR.The Ni/Co@NC hence shows an ORR activity comparable with the commercial Pt/C.

关键词： Oxygen reduction Metal-nitrogen-carbon Electrochemistry Molten salt Bimetal modulation

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P-functionalized carbon nanotubes promote highly stable electrocatalysts based on Fe-phthalocyanines for Oxygen reduction: Experimental and computational studies

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Journal of Energy Chemistry 2022年第9期31卷 276-290,I0008页

作者： Beatriz Martinez-Sanchez Diego Cazorla-Amors Emilia Morallon Departamento de Quimica Fisica and Instituto Universitario de Materiales de Alicante(IUMA)University of Alicante Ap.99.03080 AlicanteSpain Departamento de Quimica Inorganica and Instituto Universitario de Materiales de Alicante(IUMA) University of AlicanteAp.9903080 AlicanteSpain

Iron(Ⅱ) phthalocyanines(FePc) supported on functionalized nanostructured carbon materials have been studied as electrocatalysts for the Oxygen reduction reaction(ORR) in an alkaline medium. Herein, two types of carbon nanotubes(CNTs) have been explored as support, Single-Walled Carbon Nanotubes and Herringbone Carbon Nanotubes(SWCNTs and h CNTs, respectively), both electrochemically modified with ortho-aminophenylphosphonic acid(2APPA), which provides phosphate axial coordinating ligands for the immobilization of FePc molecules. All the catalysts were prepared via a facile incipient wetness impregnation method. Comprehensive experimental analysis together with density functional theory(DFT) calculations has demonstrated both the importance of the five-coordinated Fe macrocycles that favor the interaction between the FePc and the carbon support, as well as the effect of the CNT structure in the ORR. FePc axial coordination provides a better dispersion, leading to higher stability and a favorable electron redistribution that also tunes the ORR performance by lowering the stability of the reaction intermediates. Interestingly, such improvement occurs with a very low content of metal(~1 wt% Fe),which is especially remarkable when h CNT support is employed. This work provides a novel strategy for the development of Fe-containing complexes as precious metal-free catalysts towards the ORR.

关键词： Carbon nanotubes Iron phthalocyanine Oxygen reduction Electrocatalysis Axial ligand

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Electronically modulated d-band centers of MOF-derived carbon-supported Ru/HfO_(2) for Oxygen reduction and aqueous/flexible zinc-air batteries

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Journal of Energy Chemistry 2023年第5期80卷 247-255,I0007页

作者： Chuan Hu Fengli Wei Qinrui Liang Qiming Peng Yuting Yang Tayirjan Taylor Isimjan Xiulin Yang Guangxi Key Laboratory of Low Carbon Energy Materials School of Chemistry and Pharmaceutical SciencesGuangxi Normal UniversityGuilin 541004GuangxiChina Saudi Basic Industries Corporation(SABIC)at King Abdullah University of Science and Technology(KAUST) Thuwal 23955-6900Saudi Arabia

The construction of oxide/metal composite catalysts is a competent means of exploiting the electronic interactions between oxide/metal to enhance catalytic activity.In this work,we construct a novel heterogeneous composite(Ru/HfO_(2)-NC)with Ru/HfO2nanoparticles nested in nitrogen-doped porous carbon via a zeolitic imidazole frameworks-assisted(ZIF)co-precipitation and calcination approach.In particular,ZIF guides an in-situ construction of nested configuration and confines the scattered nanoparticles.Strikingly,Ru/HfO_(2)-NC exhibits unusual ORR activity,superb durability,and methanol tolerance in0.1 M KOH solution with high half-wave potential(E1/2)of 0.83 V and follows a near-4e-reaction pathway.Additionally,the ZAB assembled with cathodic Ru/HfO_(2)-NC outputs a power density of 157.3 m W cm^(-2),a specific capacity of 775 mA h g-1Zn,and a prolonged lifespan of 258 h at 5 mA cm^(-2).Meanwhile,the catalyst has demonstrated potential applicability in flexible ZAB.As suggested by experimental results and density functional theory(DFT)analysis,the remarkable property possibly originated from the optimization of the adsorption and desorption of reactive intermediates caused by the reconfiguration of the electronic structure between Ru and HfO_(2).

关键词： Ru/HfO_(2) Charge interaction oxygen vacancy Oxygen reduction Zinc-air battery

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Identifying the key N species for electrocatalytic Oxygen reduction reaction on N-doped graphene

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Nano Research 2023年第5期16卷 6642-6651页

作者： Yiyin Peng Zhaoyong Bian Wenhai Zhang Hui Wang College of Water Sciences Beijing Normal UniversityBeijing 100875China College of Environmental Science and Engineering Beijing Forestry UniversityBeijing 100083China

The state of nitrogen in nitrogen-doped graphene(NG)promoting the conversion of molecular oxygen to hydrogen peroxide was investigated.The Oxygen reduction reaction(ORR)reactivity of graphitic-N,pyrrolic-N,pyridinic-N in NG was predicted by density functional theory(DFT).A series of NG samples with different contents of these doped nitrogen types were prepared by the low-temperature thermal reduction method and used for the ORR evaluation.The H_(2)O_(2)yield,2e−ORR current efficiency,H_(2)O_(2)selectivity,electron transfer number(n)were systematically studied.The 2e−ORR selectivity was positively correlated with the N content,approaching 100%with increasing N content(0.40 V vs.reversible hydrogen electrode(RHE)),whereas the comparative energy efficiency showed a volcano-type trend related to N content,reaching a maximum of 94%.In addition,N species validation experiments proved the key role of pyrrolic-N in the synthesis of H_(2)O_(2).Compared with a pure graphene catalyst,further contaminant degradation studies on NG electrodes with different pyrrolic-N contents revealed that the lower pyrrolic-N the higher removal of p-nitrophenol(PNP).This work provides insight into the mechanism of ORR on metal-free catalysts and a facile approach to optimize this important environmental catalytic strategy.

关键词： Oxygen reduction electrocatalysis nitrogen-doped graphene environmental remediation

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Single-atomic Mn sites coupled with Fe_(3)C nanoparticles encapsulated in carbon matrixes derived from bimetallic Mn/Fe polyphthalocyanine conjugated polymer networks for accelerating electrocatalytic Oxygen reduction

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Nano Research 2022年第9期15卷 7976-7985页

作者： Yuan Pan Min Li Wanliang Mi Minmin Wang Junxi Li Yilin Zhao Xuelu Ma Bin Wang Wei Zhu Zhiming Cui Hailiang Yin Yunqi Liu State Key Laboratory of Heavy Oil Processing China University of Petroleum(East China)Qingdao 266580China Key Laboratory of Advanced Energy Materials Chemistry(Ministry of Education) College of ChemistryNankai UniversityTianjin 300071China Research Institute of Petroleum Processing SinopecBeijing 100083China School of Chemical&Environmental Engineering China University of Mining&TechnologyBeijing 100083China School of Chemistry and Chemical Engineering Shaanxi Normal UniversityXi’an 710119China State Key Lab of Organic-Inorganic Composites Beijing University of Chemical TechnologyBeijing 100029China Key Laboratory of Fuel Cell Technology of Guangdong Province South China University of TechnologyGuangzhou 510641China Academy of Science&Technology China University of Petroleum(East China)Dongying 257061China

The construction of robust coupling catalysts for accelerating electrocatalytic Oxygen reduction reaction(ORR)through the modulation of the electronic structure and local atomic configuration is critical but remains challenging.Herein,we report a facile and effective isolation-polymerization-pyrolysis(IPP)strategy for high-precision synthesis of single-atomic Mn sites coupled with Fe_(3)C nanoparticles encapsulated in N-doped porous carbon matrixes(Mn SAs/Fe_(3)C NPs@NPC)catalyst derived from predesigned bimetallic Fe/Mn polyphthalocyanine(FeMn-BPPc)conjugated polymer networks by solid-phase reaction approach.Benefiting from the synergistic effects between the single-atomic Mn-N_(4)sites and Fe_(3)C NPs as well as the confinement effect of NPC,the Mn SAs/Fe_(3)C NPs@NPC catalyst exhibited excellent electrocatalytic activity and stability for ORR.The assembled Znair battery displayed larger power density of 186 mW·cm^(−2)than that of Pt/C+Ir/C-based battery.It also exhibits excellent stability without obvious voltage change after 106 cycles with 36 h.Combing in-situ Raman spectra with in-situ attenuated total reflectance surface-enhanced infrared absorption spectroscopy(ATR-SEIRAS)characterization results indicated that the Mn-N_(4)site as an active site for the O_(2)adsorption-activation process,which effectively facilitates the generation of key*OOH intermediates and*OH desorption to promote the multielectron reaction kinetics.Theoretical calculation reveals that the excellent electrocatalytic performance originates from the charge redistribution and the d orbital shift resulting from Mn-Fe bond,which buffers the activity of ORR through the electron reservoir capable of electron donation or releasing.This work paves a novel IPP strategy for constructing high-performance coupling electrocatalyst towards the ORR for energy conversion devices.

关键词： single atom catalyst nanoparticles electrocatalyst Oxygen reduction zinc-air battery

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Carbon-based bifunctional electrocatalysts for Oxygen reduction and oxygen evolution reactions:Optimization strategies and mechanistic analysis

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Journal of Energy Chemistry 2022年第8期31卷 234-265,I0008页

作者： Huidong Xu Jack Yang Riyue Ge Jiujun Zhang Ying Li Mingyuan Zhu Liming Dai Sean Li Wenxian Li Institute of Materials Shanghai University School of Materials Science and Engineering UNSW Materials and Manufacturing Futures InstituteUniversity of New South Wales Institute for Sustainable Energy Shanghai University School of Chemical Engineering University of New South Wales Shanghai Key Laboratory of High Temperature Superconductors

Electrocatalysts are one of the essential components for the devices of high-efficiency green energy storage and conversion,such as metal-air cells,fuel cells,and water electrolysis systems.While catalysts made from noble metals possess high catalytic performance in both Oxygen reduction reaction(ORR)and oxygen evolution reaction(OER),their scarcity and expensiveness significantly limit large-scale applications.In this regard,metal-free/non-noble metal carbon-based catalysts have become competitive alternatives to replace catalysts made of noble metals.Nevertheless,low catalytic ORR/OER performance is the challenge of carbon-based catalysts for the commercial applications of metal-air batteries.To solve the problem of poor catalytic performance,two strategies have been proposed:(1)controlling the microstructure of the catalysts to expose more active sites as the channels of rapid mass and electron transfer;and(2)reducing the reaction energy barrier by optimizing the electronic structures of the catalysts via surface engineering.Here,we review different types of bifunctional ORR/OER electrocatalysts with the activated surface sites.We focus on how the challenge can be overcome with different methods of material synthesis,structural and surface characterization,performance validation/optimization,to outline the principles of surface modifications behind catalyst designs.In particular,we provide critical analysis in the challenges that we are facing in structural design and surface engineering of bifunctional ORR/OER catalysts and indicate the possible solution for these problems,providing the society with clearer ideas on the practical prospects of noble-metal-free electrocatalysts for their future applications.

关键词： Electrocatalyst Bifunctionality Oxygen reduction oxygen evolution Carbons transition metals Surface engineering Microstructure

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Silver based single atom catalyst with heteroatom coordination environment as high performance Oxygen reduction reaction catalyst

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Nano Research 2022年第9期15卷 7968-7975页

作者： Rui Sui Xuejiang Zhang Xingdong Wang Xinyu Wang Jiajing Pei Yufeng Zhang Xuerui Liu Wenxing Chen Wei Zhu Zhongbin Zhuang State Key Lab of Organic-Inorganic Composites and Beijing Advanced Innovation Center for Soft Matter Science and Engineering Beijing University of Chemical TechnologyBeijing 100029China International Clean Energy Research Office China Three Gorges CorporationBeijing 100038China Beijing Key Laboratory of Construction Tailorable Advanced Functional Materials and Green Applications School of Materials Science and EngineeringBeijing Institute of TechnologyBeijing 100081China Beijing Key Laboratory of Energy Environmental Catalysis Beijing University of Chemical TechnologyBeijing 100029China

Ag is a potential low-cost Oxygen reduction reaction(ORR)catalyst in alkaline condition,which is important for the zinc-air batteries.Here,we report that an Ag based single atom catalyst with heteroatom coordination.Ag1-h-NPClSC,has been synthesized and shown much improved performance towards ORR by manipulating the coordination environment of the Ag center.It shows a high half wave potential(0.896 V)and a high turnover frequency(TOF)(5.9 s^(−1))at 0.85 V,which are higher than the previously reported Ag based catalysts and commercial Pt/C.A zinc-air battery with high peak power density of 270 mW·cm^(−2)is fabricated by using the Ag1-h-NPClSC as air electrode.The high performance is attributed to(1)the hollow structure providing good mass transfer;(2)the single atom metal center structure providing high utility of the Ag;(3)heteroatom coordination environment providing the adjusted binding to the ORR intermediates.Density functional theory(DFT)calculations show that the energy barrier for the formation of OOH*,which is considered as the rate determine step for ORR on Ag nanoparticles,is lowered on Ag1-h-NPClSC,thus improving the ORR activity.This work demonstrates that the well manipulated Ag based single atom catalysts are promising in electrocatalysis.

关键词： Ag single-atom heteroatom coordination Oxygen reduction zinc-air battery

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Molybdenum-doped ordered L1_(0)-PdZn nanosheets for enhanced Oxygen reduction electrocatalysis

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SusMat 2022年第3期2卷 347-356页

作者： Jiashun Liang Yu Xia Xuan Liu Fanyang Huang Jinjia Liu Shenzhou Li Tanyuan Wang Shuhong Jiao Ruiguo Cao Jiantao Han Hsing-Lin Wang Qing Li State Key Laboratory of Material Processing and Die and Mould Technology School of Materials Science and EngineeringHuazhong University of Science and TechnologyWuhanChina Department of Materials Science and Engineering Southern University of Science and TechnologyShenzhenChina School of Physics and Astronomy University of BirminghamBirminghamUK Key Laboratory of Materials for Energy Conversion Chinese Academy of Science(CAS) Department of Materials Science and EngineeringUniversity of Science and Technology of ChinaHefeiChina Institute of Coal Chemistry Chinese Academy of SciencesTaiyuanChina National Energy Center for Coal to Clean Fuels Synfuels China Co.LtdBeijingChina

Ultrathin Pd-based two-dimensional(2D)nanosheets(NSs)with tunable physicochemical properties have emerged as promising candidate for Oxygen reduction reaction(ORR).Unfortunately,structurally ordered Pd-based NSs can be hardly prepared as high temperature annealing(>600℃)is necessary for disorder to order phase transition,making it a considerable challenge for morphology control.Herein,a new class of ultrathin structurally ordered Mo-doped L1_(0)-PdZn NSs with curved geometry and abundant defects/lattice distortions is reported as an efficient Oxygen reduction electrocatalyst in alkaline solution.It is found that Mo(CO)_(6) serves as reducing agent and Mo source to generate the unique ordered 2D morphology,which leads to the significantly modified electronic structure.The developed L1_(0)-Mo-PdZn NSs exhibit excellent ORR mass activity of 2.6 A mg_(Pd)^(−1) at 0.9 V versus reversible hydrogen electrode,31.5 and 17.6 times higher than those of Pd/C and Pt/C,respectively,outperforming most of the reported Pdbased ORR electrocatalsyts.Impressively,L1_(0)-Mo-PdZn NSs is extremely stable for ORR,with only 2.3% activity loss after 10000 potential cycles.Density functional theory study suggests that ordered L1_(0) structure and Mo doping can raise the vacancy formation energy of Pd atom and thus promote the ORR stability.

关键词： electrocatalysis fuel cell nanosheeets Oxygen reduction Pd-based intermetallics

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